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However, their practical implementation is heavily hindered by intrinsic limitations, particularly sluggish reaction kinetics, inferior electrical conductivity, and severe volume expansion. To address these challenges, this review provides a systematic \u201cstructure\u2010synthesis\u2010application\u201d roadmap linking the fundamental physicochemical properties of BMSs to their macroscopic electrochemical performance. First, the crystal structures and inherent advantages of BMSs are comprehensively elucidated, providing a fundamental understanding of their electrochemical superiority. Second, to overcome the inherent limitations, the impact of diverse structural design strategies on BMS performance is explored from three dimensions, including interface optimization, surface modification, and regulating interlayer electron coupling. Subsequently, various synthesis methods tailored for these distinct structural designs are summarized, revealing correlations between process parameters and morphological evolution. Building upon this foundation, this paper comprehensively evaluates the broad applications of these optimized BMS composites in electrochemical energy systems, establishing clear structure\u2010performance relationships. Finally, current challenges are identified, and future research directions are proposed. This review aims to serve as a definitive guide to accelerate the conceptualization, optimization, and practical application of next\u2010generation BMSs.<\/jats:p>","DOI":"10.1002\/smll.75911","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T17:02:41Z","timestamp":1790528561000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bimetallic Sulfides for Next\u2010Generation Energy Systems: Structure\u2010Performance Correlations, Multidimensional Regulation, and Controllable Synthesis"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-2940-1532","authenticated-orcid":false,"given":"Guanrong","family":"Wu","sequence":"first","affiliation":[{"name":"School of Mechanical and Electrical Engineering Jingdezhen Ceramic University  Jingdezhen People's Republic of 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